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Journal of Energy Chemistry 2022年第7期31卷 388-393,I0011页

作者： Xianwen Zhang Zheng Li Bin Zeng Can Li Hongxian Han State Key Laboratory of Catalysis and Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Understanding the processes of charge generation, transfer and capture is important for the design and synthesis of efficient photocatalysts. In this work, light-induced Charge separation and effect of O_(2) on electron transfer processes in SrTiO_(3) were investigated by electron paramagnetic resonance(EPR). It was found that photoinduced electron transfer from O_(2)- to Ti^(4+) produced Ti^(3+) and O- redox radical pairs under vacuum condition. Under oxygen atmosphere, however, surface bound superoxide radicals O_(2)-were formed by electron reduction of adsorbed oxygen at initial photoirradiation stage, and quenched by the reverse electron transfer to Ti^(4+) upon further photoirradiation. Formation of long-lived Charge separation associated [Ti^(3+)---O-] species and the reversibility of surface bound superoxide radicals mediating the processes of photogenerated electrons may be accountable for the high activity of SrTiO_(3) in photocatalytic water splitting reaction.

关键词： Photocatalyst Electron paramagnetic resonance Charge separation Superoxide radicals

Nanoporous MoO_(3−x)/BiVO_(4)photoanodes promoting Charge separation for efficient photoelectrochemical water splitting

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Nano Research 2022年第8期15卷 7026-7033页

作者： Songcan Wang Boyan Liu Xin Wang Yingjuan Zhang Wei Huang Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)Xi’an Institute of Biomedical Materials&EngineeringNorthwestern Polytechnical UniversityXi’an 710072China

Owing to the relatively short hole diffusion length,severe charge recombination in the bulk of bismuth vanadate(BiVO_(4))is the key issue for photoelectrochemical water splitting.Herein,we design a nanoporous MoO_(3−x)/BiVO_(4)heterojunction photoanode to promote Charge separation.The efficient electron transport properties of oxygen deficient MoO_(3−x)and the nanoporous structure are beneficial for Charge separation,leading to a significantly enhanced PEC performance.The optimized MoO_(3−x)/BiVO_(4)heterojunction photoanode exhibits a photocurrent density of 5.07 mA·cm^(−2)for Na_(2)SO_(3)oxidation.By depositing FeOOH/NiOOH dual oxygen evolution cocatalysts to promote surface kinetics,a high photocurrent density of 4.81 mA·cm^(−2)can be achieved for PEC water splitting,exhibiting an excellent applied bias photon-to-current efficiency of 1.57%.Moreover,stable overall water splitting is achieved under consecutive light illumination for 10 h.We provide a proof of concept for the design of efficient BiVO_(4)-based heterojunction photoanodes for stable PEC water splitting.

关键词： water splitting bismuth vanadate heterojunction oxygen vacancies Charge separation

Tip-induced directional Charge separation on one-dimensional BiVO4 nanocones for asymmetric light absorption

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Journal of Energy Chemistry 2022年第9期31卷 326-332,I0009页

作者： Nengcong Yang Ruotian Chen Chenwei Ni Dongfeng Li Qi Sun Lifang Liu Yu Qi Shengye Jin Xiuli Wang Fengtao Fan Can Li Fuxiang Zhang State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsDalian National Laboratory for Clean EnergyChinese Academy of SciencesDalian 116023LiaoningChina State Key Laboratory of Molecular Reaction Dynamics and Dynamics Research Center for Energy and Environmental Materials Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

One dimensional(1D)semiconductor is a class of extensively attractive materials for many emerging solar energy conversion technologies.However,it is still of shortage to assess the impact of 1D structural symmetry on spatial Charge separation and understand its underlying mechanism.Here we take controllably-synthesized 1D BiVO_(4)nanocones and nanorods as prototypes to study the influence of 1D symmetry on Charge separation.It is found that the asymmetric BiVO_(4)nanocones enable more effective Charge separation compared with the symmetric nanorods.The unexpected spatial Charge separation on the nanocones is mainly ascribed to uneven light absorption induced diffusion-controllable Charge separation due to symmetry breaking of 1D nanostructure,as evidenced by spatial and temporal resolved spectroscopy.Moreover,the promotion effect of Charge separation on the nanocones was quantitatively evaluated to be over 20 times higher than that in BiVO_(4)nanorods.This work gives the first demonstration of the influence of 1D structural symmetry on the Charge separation behavior,providing new insights to design and fabricate semiconductor materials for efficient solar energy conversion.

关键词： Charge separation Tip-enhanced light absorption Surface photovoltage BiVO4 Photocatalysis

Efficient Charge separation in hierarchical NiS@ZnIn_(2)S_(4) hollow nanospheres for photocatalytic water splitting

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Chinese Chemical Letters 2022年第2期33卷 926-929页

作者： Kai Wu Liang Mao Xiuquan Gu Xiaoyan Cai Yulong Zhao School of Materials Science and Physics China University of Mining and TechnologyXuzhou 221116China Jiangsu Province Engineering Laboratory of High Efficient Energy Storage Technology and Equipment China University of Mining and TechnologyXuzhou 221116China

In this work,hierarchical Ni S@Zn In_(2)S_(4) heterostructure was developed by constructing ultra-thin Zn In;S;(ZIS) nanosheets on hollow Ni S nanospheres for hydrogen production from photocatalytic water splitting.The Ni S@ZIS displayed a strong optical absorption ability in the visible region and a high specific surface area of 33.14 m^(2)/g.The Type-I band alignment in Ni S@ZIS heterostructure was determined by the combination of UV–vis absorption spectroscopy and Mott-Schottky curves.The photocatalytic hydrogen production of Ni S@ZIS (1.24 mmol g;h;) was nearly 5.6 times higher than that of ZIS under visible light,in the absence of any co-catalyst and sacrificial agent.The separation and migration of charge in Ni S@ZIS were characterized by a series of spectroscopy and photo/electrochemical tests,which verified the efficient charge transfer from ZIS to Ni S.

关键词： Hollow sphere Heterostructure Photocatalyst Charge separation Hydrogen production

Achieving simultaneous Cu particles anchoring in meso-porous TiO_(2) nanofabrication for enhancing photo-catalytic CO_(2) reduction through rapid Charge separation

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Chinese Chemical Letters 2022年第3期33卷 1313-1316页

作者： Jinyan Xiong Mengmeng Zhang Mengjie Lu Kai Zhao Chao Han Gang Cheng Zhipan Wen College of Chemistry and Chemical Engineering Hubei Key Laboratory of Biomass Fibers and Ecodyeing&FinishingWuhan Textile UniversityWuhan 430200China School of Chemistry and Environmental Engineering Wuhan Institute of TechnologyWuhan 430205China School of Materials Science and Energy Engineering Foshan UniversityFoshan 528000China Australia School of Civil and Environmental Engineering Faculty of Engineering and Information TechnologyUniversity of Technology SydneySydneyNSW 2007Australia

A facile solvo-thermal approach was successfully employed to prepare titanium oxide (TiO_(2)) nano-aggregates with simultaneous copper particles anchoring. The as-synthesized composite could convert CO_(2) into CH_(4) and CO products under simulated solar irradiation. The impact of copper loading amounts on the photo-reduction capability was evaluated. It was found proper amount of Cu loading could enhance the activity of CO_(2) photo-reduction. As a result, the optimal composite (TiO_(2)^(-)Cu-5%) consisting of TiO_(2) supported with 5% (mole ratio) Cu exhibits 2.2 times higher CH_(4) yield and 3 times higher CO yield compared with pure TiO_(2). Conduction band calculated from the band gap and valence X-ray photoelectron spectroscopy (XPS) indicated TiO_(2) nano-aggregates have suitable band edge alignment with respect to the CO_(2)/CH_(4) and CO_(2)/CO redox potential. Furthermore, with involving of Cu particles, an efficient separation of photo-generated charges was achieved on the basis of photocurrent response and photoluminescence spectra results, which contributed to the improved photo-catalytic performance. The present work suggested that the Cu-decorated TiO_(2) could serve as an efficient photo-catalyst for solar-driven CO_(2) photo-reduction.

关键词： TiO_(2) Copper Photo-catalytic CO_(2)reduction Photo-catalysis Charge separation Schottky junction

Surface defect-rich ceria quantum dots anchored on sulfur-doped carbon nitride nanotubes with enhanced Charge separation for solar hydrogen production

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Journal of Energy Chemistry 2021年第1期30卷 51-59,I0003页

作者： Mengru Li Changfeng Chen Liping Xu Yushuai Jia Yan Liu Xin Liu Institute of Advanced Materials College of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang 330022JiangxiChina

Designing defect-engineered semiconductor heterojunctions can effectively promote the charge carrier separation.Herein,novel ceria(CeO2) quantum dots(QDs) decorated sulfur-doped carbon nitride nanotubes(SCN NTs) were synthesized via a thermal polycondensation coupled in situ depositionprecipitation method without use of template or surfactant.The structure and morphology studies indicate that ultrafine CeO2 QDs are well distributed inside and outside of SCN NTs offering highly dispersed active sites and a large contact interface between two components.This leads to the promoted formation of rich Ce^(3+) ion and oxygen vacancies as confirmed by XPS.The photocatalytic performance can be facilely modulated by the content of CeO2 QDs introduced in SCN matrix while bare CeO2 does not show activity of hydrogen production.The optimal catalyst with 10% of CeO2 loading yields a hydrogen evolution rate of 2923.8 μmol h-1 g-1 under visible light,remarkably higher than that of bare SCN and their physical mixtures.Further studies reveal that the abundant surface defects and the created 0 D/1 D junctions play a critical role in improving the separation and transfer of charge carriers,leading to superior solar hydrogen production and good stability.

关键词： Photocatalytic hydrogen evolution Ceria quantum dots Sulfur-doped carbon nitride nanotubes Surface defects Charge separation

Promoting the Charge separation and photoelectrocatalytic water reduction kinetics of Cu_(2)O nanowires via decorating dual-cocatalysts

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Journal of Materials Science & Technology 2021年第3期62卷 119-127页

作者： Mengmeng Zhang Jiajun Wang Yang Wang Jinfeng Zhang Xiaopeng Han Yanan Chen Yuesheng Wang Zaghib Karim Wenbin Hu Yida Deng School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin300072China Center of Excellence in Transformation Electrification and Energy Storage Hydro-Québec1806 Boulevard Lionel-BouletVarennesQuébecJ3X 1S1Canada Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou350207China

Developing high activity and low-cost materials to produce hydrogen by the sustainable way of photoelectrochemical is key to social development.The abundance and inexpensive Cu_(2)O has been received increasing research as its suitable energy level for photocatalytic water reduction.However,the fast charge recombination rate and the sluggish catalytic kinetics are the huge challenges facing the Cu_(2)O photoreduction.Here,the highly reactive Cu_(2)O@C-MoS_(2)photocathode is constructed by depositing dual-cocatalysts of the carbon layer and MoS_(2)nanosheets on Cu_(2)O nanowires to realize efficient water reduction.An impressive carrier concentration of 6.59×10^(23)cm^(-3)is received,which is 2.78 times of the bare Cu_(2)O,resulting in remarkable enhancement in photocurrent density of 3.34 times for the Cu_(2)O@CMoS_(2)photocathode.Moreover,the applied bias photon-to-current conversion efficiency of the bare Cu_(2)O enhanced 4.5 times from 0.16%to 0.72%in the Cu_(2)O@C-MoS_(2)photocathode.The analysis shows that the Cu_(2)O as light absorber,the carbon layer as electron transfer promoter,and MoS_(2)nanosheets as catalytic sites,thus facilitating chrage separation and enhancing catalytic kinetics.This system paves a feasible strategy for designing other photoelectrodes to realize efficient Charge separation and high catalytic activity.

关键词： Photoelectrochemical water reduction Cu_(2)O nanowires Dual-cocatalysts modification Photocathode Charge separation

Construction of NH2-MIL-125(Ti)/Bi2WO6 composites with accelerated Charge separation for degradation of organic contaminants under visible light irradiation

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Green Energy & Environment 2020年第2期5卷 203-213页

作者： Sheng Yin Yong Chen Ming Li Qingsong Hu Yi Ding Yifan Shao Jun Di Jiexiang Xia Huaming Li School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu University301 Xuefu RoadZhenjiang 212013China School of Ecological and Environmental Science Shanghai Key Laboratory for Urban Ecological Processes and Eco-RestorationEast China Normal UniversityShanghai 200241China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore

Photocatalysis is considered as an ideal strategy for water pollution treatment.However,it remains challenging to design a highly efficient photo-catalytic system through regulating the charge flow via a precise approach.In this work,a novel NH2-MIL-125(Ti)/Bi2WO6 composite was constructed via self-assembly growing Bi2WO6 nanosheets on NH2-MIL-125(Ti)material.The characterization results demonstrated that NH2-MIL-125(Ti)was successfully incorporated into Bi2WO6 and the photoexcited carriers could be efficiently separated and transferred between the two components.NH2-MIL-125(Ti)/Bi2WO6 composites displayed enhanced photocatalytic activity for the removal of rhodamine B(RhB)and tetracycline(TC)under visible light irradiation,and the optimal weight ratio of NH2-MIL-125(Ti)was determined to be 7 wt%.The introduction of NH2-MIL-125(Ti)into Bi2WO6 could raise the absorption of visible light,accelerate the separation and transfer of charge carriers,and boost photocatalytic activity.This research presents a wide range of possibilities for the further development of novel composites in the field of environment purification.

关键词： NH2-MIL-125(Ti) Bi2WO6 nanosheets Charge separation Photocatalysis Visible light

Modulating Charge separation and transfer kinetics in carbon nanodots for photoredox catalysis

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Journal of Energy Chemistry 2020年第11期29卷 365-377页

作者： Pengju Yang Zhidong Yang School of Chemistry and Chemical Engineering Shanxi UniversityTaiyuan 030006ShanxiChina

Artificial photosynthesis has gained increasing interest as a promising solution to the worldwide energy and environmental issues. A crucial requirement for realizing a sustainable system for artificial photosynthesis is to explore low cost, highly-efficient and stable photoactive materials. Carbon nanodots(CNDs) have attracted considerable attention owing to their low cost, tunable chemistry and unique light-harvesting capability. Previous review articles have highlighted the photocatalytic and photoelectrocatalytic applications of CNDs and CNDs-based composite photocatalysts. However, the control of the separation and transfer processes of photogenerated electron/hole pairs in CNDs has not been reviewed.This review summarizes the recent progress in the design of CNDs as new light-harvesting materials and highlights their applications in photocatalytic hydrogen production, CO2 photoreduction and environmental remediation. Strategies that have been employed to modulate the separation and transfer kinetics of photogenerated charge carriers in CNDs are discussed in detail. The challenges and new directions in this emerging area of research are also proposed.

关键词： Carbon nanodot Artificial photosynthesis Charge separation Visible light

Suitable energy platform significantly improves Charge separation of g-C3N4 for CO2 reduction and pollutant oxidation under visible-light

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Progress in Natural Science:Materials International 2019年第2期29卷 138-144页

作者： Amir Zada Nauman Ali Fazle Subhan Natasha Anwar Muhammad Ishaq Ali Shah Muhammad Ateeq Zahid Hussain Khair Zaman Momin Khan Department of Chemistry Abdul Wali Khan University Key Laboratory of Functional Inorganic Materials Chemistry (Heilongjiang University) Ministry of Education School of Chemistry and Materials Science International Joint Research Center for Catalytic Technology Institute of Chemical Sciences University of Peshawar

The photocatalytic activities of g-C3N4can be significantly improved by increasing life time of the photogenerated charges. Here, in this work we introduced TiO2as proper energy platform to accept the photogenerated electrons from g-C3N4during photocatalysis. The nanophotocatalysts formed from the combination of a suitable amount of TiO2nanoparticles and g-C3N4nanosheets showed 8.75 and 4.22% enhancement in photocatalytic activities for CO2reduction and 2-chlorophenol(2-CP) degradation under visible light illumination as compared to bare g-C3N4. Based on the surface photovoltage spectra, photoluminescence spectra and examination of formed hydroxyl radicals, it was confirmed that these enhanced photoactivities were attributed to the much-improved Charge separation via the electron transfer from g-C3N4to TiO2. From trapping experiments,it was found that hydroxyl radicals were the major species involved in the photocatalytic degradation of 2-CP.This study is helpful to synthesize efficient photocatalysts to cope with energy and environmental issues.

关键词： Nanophotocatalyst Charge separation CO2 reduction Pollutant degradation